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Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime

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Abstract

We present a theoretical description of double-pump femtosecond single-molecule signals with fluorescence detection. We simulate these signals in the weak-field regime for a model mimicking a chromophore with a Franck–Condon-active vibrational mode. We establish several signatures of these signals which are characteristic for the weak-field regime. The signatures include the quenching of vibrational beatings by electronic dephasing and a pronounced tilt of the phase-time profiles in the two-dimensional (2D) maps. We study how environment-induced slow modulations of the electronic dephasing and relevant chromophore parameters (electronic energy, orientation, vibrational frequency and relative shift of the potential energy surfaces) affect the signals.

Graphical abstract: Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime

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Publication details

The article was received on 17 Jul 2017, accepted on 20 Nov 2017 and first published on 20 Nov 2017


Article type: Paper
DOI: 10.1039/C7CP04809B
Citation: Phys. Chem. Chem. Phys., 2017, Advance Article
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    Theoretical aspects of femtosecond double-pump single-molecule spectroscopy. I. Weak-field regime

    E. Palacino-González, M. F. Gelin and W. Domcke, Phys. Chem. Chem. Phys., 2017, Advance Article , DOI: 10.1039/C7CP04809B

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